Biomass waste is a valuable resource that can be recovered, reused, and is renewable. However, converting biomass waste to a high degree of order is a bigger challenge, and graphitization at low temperatures is even more difficult. This paper proposes an improved method (Ni element catalysis) for highly graphitizing pomelo peel at low temperatures (750 –900 °C). In this paper, X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), and high-resolution transmission electron microscopy (HRTEM) were used to study the method and the effect of temperature on structural changes during graphitization. Under the improved method, pomelo peel was transformed into nano-spherical graphitized material. The degree of graphitization reached 80.23% at 900 °C, which was 31.39% higher than that of the traditional method. Furthermore, through HRTEM, the lattice fringe spacing was observed to be 0.337 nm, which is between pure graphite (0.3354 nm) and amorphous graphite (0.3440 nm). In this paper, the improved method can obtain highly graphitized nanospheres at low temperatures, thus reducing energy consumption, reducing environmental pollution, and promoting sustainable development.